Mechanism of Zn salt-induced deactivation of a Cu/activated carbon catalyst for low-temperature denitration via CO-SCR
2022
Wen, Zhenjing | Huang, Bangfu | Shi, Zhe | Yang, Zhengyu | Dai, Meng | Li, Wanjun | Zi, Gaoyong | Luo, Liubin
In the process of industrial flue gas denitration, the presence of heavy metals, especially Zn salts, is known to lead to the deactivation of the denitration catalysts. However, the specific mechanism of the catalyst deactivation remains unclear. In this paper, the mechanism of the ZnCl₂- and ZnSO₄-induced deactivation of low-temperature denitration catalysts in the carbon oxide (CO) selective catalytic reduction (CO-SCR) reaction was investigated using a Cu/activated carbon (AC) catalyst, in which HNO₃/AC was used as the carrier. Cu/AC, ZnCl₂–Cu/AC, and ZnSO₄–Cu/AC catalysts were prepared by the incipient wetness impregnation method. The physicochemical properties of the catalyst were examined via the Brunauer–Emmett–Teller method, X-ray diffraction, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy analyses, which proved the mechanism of catalyst denitrification and enabled the elucidation of the toxicity mechanism of the Zn salts on the Cu/AC catalyst for CO-SCR denitration at low temperatures. The results show that Zn doping reduces the physical adsorption of CO and NO and decreases the concentration of Cu²⁺ and chemisorbed oxygen (Oᵦ), leading to the reduction of active sites and oxygen vacancies, thus inhibiting the denitration reaction. Moreover, ZnCl₂ is more toxic than ZnSO₄ because Cl⁻ not only occupies oxygen vacancies but also inhibits Oᵦ migration. In contrast, SO₄²⁻ increases the surface acidity and promotes Oᵦ supplementation. This study can provide a reference for the development of CO-SCR denitration catalysts with high resistance to Zn salt poisoning.
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